CN108636069B - A method for membrane electrolysis to promote electrochemical capture of low-concentration CO2 - Google Patents
A method for membrane electrolysis to promote electrochemical capture of low-concentration CO2 Download PDFInfo
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- 238000000034 method Methods 0.000 title claims abstract description 71
- 238000005868 electrolysis reaction Methods 0.000 title claims abstract description 64
- 239000012528 membrane Substances 0.000 title claims abstract description 17
- 238000006243 chemical reaction Methods 0.000 claims abstract description 49
- 230000005518 electrochemistry Effects 0.000 claims abstract description 30
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 19
- 238000005341 cation exchange Methods 0.000 claims abstract description 12
- 238000010521 absorption reaction Methods 0.000 claims abstract description 9
- 230000009471 action Effects 0.000 claims abstract description 4
- 229910052921 ammonium sulfate Inorganic materials 0.000 claims description 21
- 239000001257 hydrogen Substances 0.000 claims description 21
- 229910052739 hydrogen Inorganic materials 0.000 claims description 21
- 239000003115 supporting electrolyte Substances 0.000 claims description 20
- 238000003795 desorption Methods 0.000 claims description 16
- 239000003792 electrolyte Substances 0.000 claims description 14
- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 claims description 13
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 12
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 10
- 239000007788 liquid Substances 0.000 claims description 10
- 150000002431 hydrogen Chemical group 0.000 claims description 9
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 8
- 239000000908 ammonium hydroxide Substances 0.000 claims description 8
- 238000009792 diffusion process Methods 0.000 claims description 8
- 239000006260 foam Substances 0.000 claims description 5
- 229910052759 nickel Inorganic materials 0.000 claims description 5
- 230000005611 electricity Effects 0.000 claims description 3
- 238000005265 energy consumption Methods 0.000 abstract description 22
- 239000000126 substance Substances 0.000 abstract description 5
- 238000012423 maintenance Methods 0.000 abstract description 2
- 239000007789 gas Substances 0.000 description 28
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 25
- 230000008569 process Effects 0.000 description 19
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 13
- 230000036647 reaction Effects 0.000 description 11
- 238000004817 gas chromatography Methods 0.000 description 9
- HZAXFHJVJLSVMW-UHFFFAOYSA-N 2-Aminoethan-1-ol Chemical compound NCCO HZAXFHJVJLSVMW-UHFFFAOYSA-N 0.000 description 8
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 6
- 239000002250 absorbent Substances 0.000 description 6
- 230000002745 absorbent Effects 0.000 description 6
- 238000005516 engineering process Methods 0.000 description 6
- 230000008929 regeneration Effects 0.000 description 6
- 238000011069 regeneration method Methods 0.000 description 6
- 238000000354 decomposition reaction Methods 0.000 description 4
- 239000003546 flue gas Substances 0.000 description 4
- 239000002803 fossil fuel Substances 0.000 description 4
- 238000010438 heat treatment Methods 0.000 description 4
- 239000004615 ingredient Substances 0.000 description 4
- 238000000926 separation method Methods 0.000 description 4
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 3
- 229910021529 ammonia Inorganic materials 0.000 description 3
- 229910052786 argon Inorganic materials 0.000 description 3
- 230000008901 benefit Effects 0.000 description 3
- VTYYLEPIZMXCLO-UHFFFAOYSA-L calcium carbonate Substances [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 238000002485 combustion reaction Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- USFZMSVCRYTOJT-UHFFFAOYSA-N Ammonium acetate Chemical compound N.CC(O)=O USFZMSVCRYTOJT-UHFFFAOYSA-N 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 229910000019 calcium carbonate Inorganic materials 0.000 description 2
- 238000004364 calculation method Methods 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 239000003245 coal Substances 0.000 description 2
- 238000005260 corrosion Methods 0.000 description 2
- 230000007797 corrosion Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- ZBCBWPMODOFKDW-UHFFFAOYSA-N diethanolamine Chemical compound OCCNCCO ZBCBWPMODOFKDW-UHFFFAOYSA-N 0.000 description 2
- 229940043237 diethanolamine Drugs 0.000 description 2
- 238000006460 hydrolysis reaction Methods 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- BWHMMNNQKKPAPP-UHFFFAOYSA-L potassium carbonate Chemical compound [K+].[K+].[O-]C([O-])=O BWHMMNNQKKPAPP-UHFFFAOYSA-L 0.000 description 2
- 238000005086 pumping Methods 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 230000035484 reaction time Effects 0.000 description 2
- 230000002441 reversible effect Effects 0.000 description 2
- 239000002918 waste heat Substances 0.000 description 2
- 239000005695 Ammonium acetate Substances 0.000 description 1
- ATRRKUHOCOJYRX-UHFFFAOYSA-N Ammonium bicarbonate Chemical compound [NH4+].OC([O-])=O ATRRKUHOCOJYRX-UHFFFAOYSA-N 0.000 description 1
- 229910000013 Ammonium bicarbonate Inorganic materials 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 1
- -1 H2In hydrogen Chemical class 0.000 description 1
- 239000003463 adsorbent Substances 0.000 description 1
- 229940043376 ammonium acetate Drugs 0.000 description 1
- 235000019257 ammonium acetate Nutrition 0.000 description 1
- 235000012538 ammonium bicarbonate Nutrition 0.000 description 1
- 239000001099 ammonium carbonate Substances 0.000 description 1
- 235000019270 ammonium chloride Nutrition 0.000 description 1
- 235000011130 ammonium sulphate Nutrition 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 239000000920 calcium hydroxide Substances 0.000 description 1
- 229910001861 calcium hydroxide Inorganic materials 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 238000004587 chromatography analysis Methods 0.000 description 1
- 235000019504 cigarettes Nutrition 0.000 description 1
- 238000009841 combustion method Methods 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000002955 isolation Methods 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 230000035800 maturation Effects 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
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- 229910000027 potassium carbonate Inorganic materials 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
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- 230000004044 response Effects 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 230000004083 survival effect Effects 0.000 description 1
- 238000001926 trapping method Methods 0.000 description 1
- 238000005292 vacuum distillation Methods 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
- B01D53/326—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00 in electrochemical cells
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1425—Regeneration of liquid absorbents
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1456—Removing acid components
- B01D53/1475—Removing carbon dioxide
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1493—Selection of liquid materials for use as absorbents
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/10—Inorganic absorbents
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- Engineering & Computer Science (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
The present invention provides a kind of film electrolysis promotion low concentration CO2The method of electrochemistry trapping belongs to electrochemistry trapping CO2Technical field.The method is that cation-exchange membrane is placed in electrolytic cell to be classified as anode region and cathodic region, and NH is added in anode region4HCO3Solution, cathodic region are passed through low concentration CO2, and apply DC power supply between anode electrode and cathode electrode: under the action of electric current, H of the water power from generation+With the NH in anolyte4HCO3Reaction releases the CO of high-purity2, while generating NH4 +；NH4 +The OH of cathodic region and water power from generation is reached through cation-exchange membrane‑In conjunction with generation NH3·H2O absorbs low concentration CO for capturing2, and by the NH of generation4HCO3It is recycled back to anode region.When maintenance current density is 40mA/cm2When, the starting voltage of the method for the present invention is only 0.61V, traps one ton of CO2Actual consumption be 1.575GJ, just correspond to the 45% of traditional MEA chemical absorption method energy consumption.
Description
Technical field
The invention belongs to electrochemistry to trap CO2Technical field, specially a kind of film electrolysis promote low concentration CO2Electrochemistry is caught
The method of collection.
Background technique
For a long time, a large amount of uses of fossil fuel cause CO in global range2The rapid growth of discharge amount.According to international energy
Affix one's name to the report of (IEA) publication, the CO discharged in atmosphere in 2011 by combustion of fossil fuel in source21.4 at the beginning of the 70's of last century
× 104Mt rises to 3.1 × 104Mt.The demand of " BP the year two thousand thirty world energy outlook " estimated global energy in 2011 extremely
36%, CO will be increased during the year two thousand thirty2Discharge amount will be further increased, CO2Emission reduction is not only the sciences problems of facing mankind, more
It is the big problem concerning human survival and development.
In the coming years, the energy is still mainly obtained from fossil fuel.Especially China is in the following very long period
It is interior, the basic configuration based on coal will be continued in terms of energy resource structure.Therefore, in a short time in end-o f-pipe -control combustion of fossil fuel
The CO discharged2It will be the main method for reducing carbon emission.By CO2It is caught from the fixed discharges source such as power plant and cement plant
Obtaining is CO2The first step that emission-reduction technology is carried out.Current most of coal-burning power plant all directly burns coal, therefore fires
The use scope of carbon capture technology is most wide after burning, and the technology is by CO2Separated from the flue gas discharged after fuel combustion to
Reach CO2The effect of enrichment.Carbon capture process mainly applies following technology: absorption process, absorption method, UF membrane after current combustion
Method, the separation based on hydrate and low temperature distillation etc..
Chemical absorption method has the advantages such as technology maturation, uptake be big, is generally considered most economical practical CO2It captures
Technology.This method absorbs CO first with liquid-absorbant from flue gas2.Then absorbent by removing, heat or depressurize into
Row regeneration, while discharging pure CO2, typical adsorbent includes monoethanolamine (MEA), diethanol amine (DEA) and potassium carbonate.Its
In, monoethanolamine (MEA) is CO2Trap the professional standard reagent of chemical absorption method, trapping and desorption CO2Overall reaction it is as follows:
CO2+2HOCH2CH2NH2+H2O→(HOCH2CH2NH3)2CO3
Above-mentioned reaction is reversible exothermic reaction, and under 20-40 DEG C of low-temperature condition, reaction forward is carried out, and realizes CO2Catch
It catches；Under the 110-125 DEG C of condition of high temperature, reacts reverse and carry out, desorb pure CO2And realize the regeneration of solvent MEA.At this
During a, the regenerative process of absorbent, which occupies, is mostly used in CO2The energy consumption of trapping.
The energy consumption of absorbent regeneration can be divided into three parts: for the reaction heat of solvent reclamation, for improving solution temperature
The sensible heat of degree, loss thermal energy.It is theoretically used for regenerated reaction heat and is up to 2.16GJ/t-CO2.In actual operation, then
Boiling device energy consumption is 3.2~4.0GJ/t-CO2, wherein the energy consumption accounting of heating and heat loss is close to 40%.Therefore, rich solution liter is reduced
Warm energy consumption, avoiding vapour losses is to reduce CO2Capture the key of energy consumption.
By the inspiration of chlorine industry, CO is carried out about using the method for electrochemistry2Trapping report, this method is in electricity
Water is become into O in solution preocess2And H2, and H+ and OH- is enriched in anode region and cathodic region respectively.Then the H of anode region is used+It is molten
Solve CaCO3The pure CO of output2, Ca is left in the solution2+With the OH in cathodic region-In conjunction with generation Ca (OH)2。Ca(OH)2Absorb cigarette
CO in gas2Regenerate CaCO3.Since traditional electrolyte process must be by generating H2And O2Realize entire reaction process, so that
The theoretical power consumption of the process is up to 6.048GJ/t-CO2。
Summary of the invention
It is an object of the invention to capture low concentration CO for above-mentioned existing chemical absorbing and electrochemistry2Existing high energy consumption
Problem provides a kind of film electrolysis promotion low concentration CO2The method of electrochemistry trapping.The object of the invention is come by the following technical programs
It realizes:
A kind of film electrolysis promotion low concentration CO2The method of electrochemistry trapping, including absorption and desorption:
It is described to be absorbed as under film electrolysis, ammonium hydroxide is absorbed into low concentration CO2The NH generated afterwards4HCO3As electrolyte,
It is electrolysed the NH generated4 +OH with water power from generation-In conjunction with generation NH3·H2O, circulation is as capture low concentration CO2Absorbing liquid；
The desorption is the NH under film electrolysis4HCO3It is electrolysed the HCO generated3 -H with water power from generation+In conjunction with generation
High-purity CO2。
As a kind of film electrolysis promotion low concentration CO of the present invention2One specific implementation of the method for electrochemistry trapping
Example, the method are that cation-exchange membrane is placed in electrolytic cell to be classified as anode region and cathodic region, and anode region is added
NH4HCO3Solution, cathodic region are passed through low concentration CO2, and apply DC power supply between anode electrode and cathode electrode:
Under the action of electric current, H of the water power from generation+With the NH in anolyte4HCO3Reaction releases high-purity
CO2, while generating NH4 +；NH4 +The OH of cathodic region and water power from generation is reached through cation-exchange membrane-In conjunction with generation NH3·
H2O absorbs low concentration CO for capturing2, and by the NH of generation4HCO3It is recycled back to anode region.
As a kind of film electrolysis promotion low concentration CO of the present invention2One specific implementation of the method for electrochemistry trapping
Example, the temperature of the electrolytic cell are 45~55 DEG C.
As a kind of film electrolysis promotion low concentration CO of the present invention2One specific implementation of the method for electrochemistry trapping
Example, the anode electrode are hydrogen diffusion electrode, and the cathode electrode is foam nickel electrode.
As a kind of film electrolysis promotion low concentration CO of the present invention2One specific implementation of the method for electrochemistry trapping
Example, the anode region are passed through hydrogen, and hydrogen is oxidized to H on the anode electrode+。
As a kind of film electrolysis promotion low concentration CO of the present invention2One specific implementation of the method for electrochemistry trapping
Example, the hydrogen is precipitated by cathodic region, and is recycled back to cathodic region by hydrogen storage tank.
As a kind of film electrolysis promotion low concentration CO of the present invention2One specific implementation of the method for electrochemistry trapping
Example, the anode region and cathodic region also need that supporting electrolyte (NH is added4)2SO4。
As a kind of film electrolysis promotion low concentration CO of the present invention2One specific implementation of the method for electrochemistry trapping
Example, the anode region (NH4)2SO4, cathodic region (NH4)2SO4And anode region electrolyte NH4HCO3Molar concentration rate be 1:1:
1。
As a kind of film electrolysis promotion low concentration CO of the present invention2One specific implementation of the method for electrochemistry trapping
Example, the low concentration CO2Concentration be 10~20%, the high-purity CO2Concentration be 100%.
As a kind of film electrolysis promotion low concentration CO of the present invention2One specific implementation of the method for electrochemistry trapping
Example, anode region, cathodic region solution using the storage of corresponding solution reservoir, and make solution in anode region, cathode by circulating pump
It is recycled between area and corresponding storage tank.
Compared with prior art, the invention has the following advantages:
It is electrolysed present invention firstly provides film and promotes low concentration CO2The method of electrochemistry trapping, utilizes film electrolysis tech energy
Efficiently promote NH4HCO3Double hydrolysis, make low concentration CO2It is converted into high-purity CO2.In the method for the present invention, anode region is generated
H+With HCO3 -CO is realized in reaction2Desorption；The OH that cathodic region generates-With NH4 +Reaction is NH3·H2O facilitates absorbent
Regeneration；To realize CO respectively under isothermal, low energy consumption2The process of desorption and solvent reclamation avoids the same of heating energy consumption
When reduce CO2The reaction heat of desorption.
When maintenance current density is 40mA/cm2When, the starting voltage of the method for the present invention is only 0.61V, absorbent regeneration and
CO2The current efficiency of desorption is respectively 98.2% and 98.5%.Trap one ton of CO2Actual consumption be 1.575 GJ, just correspond to
Traditional MEA chemical absorption method energy consumption (3.5GJ/t-CO2) 45%.
Detailed description of the invention
Fig. 1 is that film electrolysis promotes low concentration CO2The operation principle schematic diagram of electrochemistry trapping.
Fig. 2 is that the GC of cell reaction front and back membrane electrolysis cells exit gas detects ingredient as a result, wherein a indicates anode region, b
Indicate cathodic region.
Fig. 3 is 1 current density of example in 40mA/cm2The relationship that tank voltage changes with the reaction time when being electrolysed.
Fig. 4 is that 1 current density of example is 40mA/cm2Shi Sanci recycle completely after experimental result.
U-I curve when Fig. 5 being 15 DEG C using different supporting electrolytes.
(the NH of various concentration when Fig. 6 is 15 DEG C4)2SO4U-I curve as supporting electrolyte.
Fig. 7 is the U-I curve under different temperatures.
Specific embodiment
In order to make the objectives, technical solutions, and advantages of the present invention clearer, with reference to the accompanying drawings and embodiments, right
The present invention is further elaborated.It should be appreciated that the specific embodiments described herein are merely illustrative of the present invention, and
It is not used in the restriction present invention.
A kind of film electrolysis promotion low concentration CO2The method of electrochemistry trapping, including absorption and desorption:
It is described to be absorbed as under film electrolysis, ammonium hydroxide is absorbed into low concentration CO2The NH generated afterwards4HCO3As electrolyte,
It is electrolysed the NH generated4 +OH with water power from generation-In conjunction with generation NH3·H2O, circulation is as capture low concentration CO2Absorbing liquid；
The desorption is the NH under film electrolysis4HCO3It is electrolysed the HCO generated3 -H with water power from generation+In conjunction with generation
High-purity CO2。
Ammonium hydroxide is to CO2Absorptive capacity be far longer than MEA.Therefore, in the method for the present invention, we introduce ammonium hydroxide as CO2It inhales
Receive agent.Firstly, ammonium hydroxide is absorbed CO2The NH generated afterwards4HCO3It is introduced into membrane electrolysis cells as electrolysis raw material, is containing NH4HCO3
The power-up of system China and foreign countries can break the ionization equilibrium of water, to promote NH4HCO3Hydrolysis separation.The process makes NH4 +With water power
OH from generation-CO can be efficiently captured in conjunction with generating2NH3·H2O, while by HCO3 -The H separated out with water power+In conjunction with release
Pure CO2.The method of the present invention is just able to achieve CO under isothermal conditions2Capture and separation, avoid traditional heating realize CO2Desorption
Energy consumption caused by process；Meanwhile the introducing of film electrolysis tech significantly reduces the high energy consumption of electrolytic process.
Specifically, the specific implementation of the above method are as follows:
Cation-exchange membrane is placed in electrolytic cell and is classified as anode region and cathodic region, NH is added in anode region4HCO3It is molten
Liquid, cathodic region are passed through low concentration CO2, and apply DC power supply between anode electrode and cathode electrode:
Under the action of electric current, H of the water power from generation+With the NH in anolyte4HCO3Reaction releases high-purity
CO2, while generating NH4 +；NH4 +The OH of cathodic region and water power from generation is reached through cation-exchange membrane-In conjunction with generation NH3·
H2O absorbs low concentration CO for capturing2, and by the NH of production4HCO3It is recycled back to anode region.
Further, the temperature of the electrolytic cell is 45~55 DEG C.
Further, the anode electrode is hydrogen diffusion electrode, and the cathode electrode is foam nickel electrode.
Further, the anode region is passed through hydrogen, and hydrogen is oxidized to H on the anode electrode+。
Further, the hydrogen is precipitated by cathodic region, and is recycled back to cathodic region by hydrogen storage tank.
Film electrolysis promotes CO2The method of capture has reached promotion NH by breaking the ionization equilibrium of water4HCO3The mesh of decomposition
, make NH4 +For absorbing low concentration CO2NH3·H2O and for desorbing high concentration CO2NH4HCO3Between convert, and
It is final to realize low concentration CO2It is changed into high concentration CO2Process:
Overall reaction: low concentration CO2(10%~20%) → high-purity CO2(100%) (1)
Fig. 1 is that film electrolysis promotes low concentration CO2The operation principle schematic diagram of electrochemistry trapping.Cation-exchange membrane will be electrolysed
Slot is divided into cathodic region and anode region, and hydrogen diffusion electrode is as anode, and nickel foam is as cathode.Under the function of current, H2In hydrogen
H is oxidized on gas diffusion electrode+(reaction 2), and with the NH in anolyte4HCO3Reaction discharges CO2(purity 100%)
NH is generated simultaneously4 +(reaction 3).Hydrogen is precipitated in cathodic region simultaneously, OH-In cathodic enrichment (reaction 4).In order to reach in electrolytic cell
The charge balance in portion, NH4 +Cathodic region and OH are reached through cation-exchange membrane-In conjunction with generation NH3·H2O (reaction 5).Electrolysis life
At NH3·H2O is for absorbing low concentration CO2(reaction 6), and the NH that reaction is generated4HCO3It is placed in anode region, circulation carries out anti-
Answer 2.
Anode region: H2-2e-→2H+ (2)
NH4HCO3+H+→CO2(100%)+NH4 ++H2O (3)
Cathodic region: H2O+2e-→2OH-+H2 (4)
OH-+NH4 +→NH3·H2O (5)
Low concentration CO2It absorbs: CO2(10%~20%)+NH3·H2O→NH4HCO3 (6)
Further, the anode region and cathodic region also need that supporting electrolyte (NH is added4)2SO4.In membrane electrolysis cells, according to
By ionic conduction current, therefore good solution conductivity promotes cell reaction most important the efficient operation of membrane electrolysis cells.
Supporting electrolyte, which is added, can be improved the ion concentration of electrolyte in entire membrane electrolysis cells, to accelerate the transmission of electric current, accelerate
The progress of entire reaction process.
Further, the anode region supporting electrolyte (NH4)2SO4, cathodic region supporting electrolyte (NH4)2SO4And anode
Area electrolyte NH4HCO3Molar concentration rate be 1:1:1.Excessively high (NH4)2SO4Concentration will affect ammonium hydroxide and absorb CO2It generates
NH4HCO3Reaction balance, cause unit volume absorb CO2Amount reduce, too low (NH4)2SO4Concentration cannot reach increase electricity
Solve the purpose that liquid ion concentration improves electric current transmission.
Heretofore described low concentration CO2Concentration be 10~20%, the high-purity CO2Concentration be 100%.
Further, the solution in anode region of the present invention, cathodic region is using the storage of corresponding solution reservoir, and is made by circulating pump
Solution recycles between anode region, cathodic region and corresponding storage tank.
Low concentration CO is promoted to a kind of present invention film electrolysis below with reference to specific example2Electrochemistry trapping method carry out into
One step explanation.
Raw material employed in example and source are as follows:
Analytically pure ammonium sulfate, ammonium chloride, ammonium acetate, ammonium hydrogen carbonate are used directly as experimental raw.Purity is 99.99%
H2With Ar and CO2+N2Mixed gas (CO2: 15%；N2: 85%) it buys to east wind (Sichuan) gas companies.It supports
1mg/cm2Pt/C catalyst the purchase of hydrogen diffusion electrode from gloomy (Shanghai) company in river, cation-exchange membrane uses
Nafion115 film (E.I.Du Pont Company), nickel foam is used as cathode electrode.
Example 1
Cation-exchange membrane Nafion115 film is placed in electrolytic cell, electrolytic cell is divided into cathodic region and anode region, anode
Liquid (1M (NH4)2SO4+1MNH4HCO3) and catholyte (1M (NH4)2SO4) be placed in the closed storage tank of 200mL, it is being electrolysed by pump
With the flow velocity circulation of 20mL/min between slot device and storage tank, and it is passed through to anode region the H of 10mL/min2.Anode electrode
Apply DC power supply between cathode electrode, cell reaction is powered using external dc power supply (IT6932A, Itech), electrolytic cell
Temperature is 50 DEG C.
Current density is set as 40mA/m2, and constantly monitor and record the voltage change rule of electrolytic cell.Electrolytic process
In, the CO that the argon gas of 20mL/min will desorb in anolyte is passed through into anode liquid storage tank2It carries into gas-chromatography, verifying
That desorb is CO2Anode output CO is detected while gas2Purity.Simultaneously by low concentration CO2 (CO2=15%, N2=
85%) it is passed through in catholyte with the speed of 5mL/min and carries out CO2Absorbing reaction, and CO will be absorbed2Tail gas afterwards is passed through gas phase
In chromatography, verifying cathode generates and can be used to absorb CO2Ammonia spirit.
In electrolytic process, the purpose of core is to absorb low concentration CO2And output high concentration CO2.In order to verify film electrolytic process
Whether there is CO2Capture and isolated effect, during the experiment, before and after gas-chromatography is for measuring film cell reaction, yin, yang
The composition of pole exit gas changes.
Fig. 2 is that the GC of cell reaction front and back membrane electrolysis cells exit gas detects ingredient as a result, wherein a indicates anode region； b
Indicate cathodic region.From figure 2 it can be seen that anode region is passed through Ar and is connected in gas-chromatography before film cell reaction starts,
It finds no any gas peak and occurs (note: Ar not appearance).After impressed current starts reaction, apparent CO can detecte2
Peak, and and be not detected other gas appearances (see Fig. 2 a), it was demonstrated that anode region produces CO2And its purity reaches 100%, together
When also demonstrate the film electrolytic process of the application and can effectively realize CO2Desorption reaction.And before film cell reaction starts, cathode
Area is passed through low concentration CO2Gas is simultaneously connected to gas chromatograph, the CO of internal mark method determination2Concentration is 15%, remaining component is all N2
(85%).After cell reaction starts, CO in cathode outlet gas2Relative amount be greatly reduced, be detected simultaneously by H2Life
At (see Fig. 2 b).Testing result meets expected film electrolysis and promotes CO2The reaction principle of trapping, it was demonstrated that film electrolysis tech is applied to
CO2The feasibility of trapping.
Energy consumption analysis
Film electrolysis promotes CO2The electrolysis energy consumption (W) and tank voltage (U) of trapping and the following (formula of the relationship of current efficiency (η)
7):
Wherein q indicates CO2Electrochemical equivalent, electrochemical equivalent q=1.64145g/ (Ah), quality m unit be kg,
η is the current efficiency of electrolytic process.
Fig. 3 is this example current density in 40mA/cm2The relationship that tank voltage changes with the reaction time when being electrolysed.From
In figure as can be seen that when current density is 40mA/cm2When, starting voltage 0.61V.After starting electrolysis, the fluctuation of voltage is compared
Seriously, with the progress of reaction, voltage fluctuation is gradually reduced.This is because CO2It is constantly raw on the surface of hydrogen diffusion electrode
At and desorption, the stability of anode electrode is affected, with HCO in anolyte3 -It is constantly consumed, CO2Quantum of output gradually decreases
To not output, become smaller to the interference of gas-diffusion electrode, so that voltage be made tend towards stability with reaction.
It brings the test data of Fig. 3 into calculating that formula 7 carries out electrolysis energy consumption, captures CO per ton2Electrolysis energy consumption be
437.615kWh (1.575GJ) only uses CO of the MEA as absorbent at present2The energy consumption of trapping and isolation technics
The 45% of (3.5GJ).
The cyclical stability of film electrolytic process is tested
It is electrolysed in film and promotes CO2In the method for trapping, after applying electric current, the NH of anode region4HCO3CO can occur2Desorption
Reaction, cathodic region can generate NH3·H2O.By the NH of generation3·H2O is for absorbing CO2It is changed into NH4HCO3, generation
NH4HCO3It is passed through anode region desorption CO again2, circulation realizes CO according to this2Trapping with separate.Therefore, the circulation of film electrolytic process
Stability is most important to the implementation of the method for the present invention.
As the HCO in anolyte3 -After concentration is reduced to 0.214M, stop cell reaction.And by electrolyte respectively from
It is pumped out in electrolytic cell, contains NH in electrolytically generated3·H2CO is passed through in the catholyte of O2, it is changed into containing NH4HCO3It is molten
Liquid is pumped into anolyte of the anode region of electrolytic cell as circular response next time.By HCO3 -Anolyte after concentration reduces is passed through
Cathodic region is as the catholyte recycled next time.It constantly recycles by this method, and passes through the voltage change in measurement reaction process
Determine that repeatedly the electrolysis of circulation caudacoria promotes CO2The reaction stability of trapping.It in current density is 40mA/cm that Fig. 4, which is this example,2When
Experimental result completely after circulation three times.It can be seen from the figure that film electrolysis promotes CO2The process of trapping has very high circulation
Power of regeneration, three times compared with starting voltage (0.61V) of the starting voltage (0.62V) after circulation when first time circulation not
It changes significantly.Therefore CO is carried out using well-behaved inventive method2Trapping and separation have steadily in the long term run a possibility that.
Example 2
By anolyte (1.5M (NH4)2SO4+1.5MNH4HCO3) and catholyte (1.5M (NH4)2SO4) it is placed in the close of 200mL
It closes in storage tank, by pumping between electrolytic cell assembly and storage tank with the flow velocity circulation of 15mL/min, and is passed through to hydrogen area
The H of 10mL/min2.Apply DC power supply between anode electrode and cathode electrode, cell reaction uses external dc power supply
(IT6932A, Itech) power supply, electrolyzer temperature are 55 DEG C.
Current density is set as 20mA/m2, decomposition voltage at this time is 0.53V.Therefore, according to formula (7) calculation shows that:
Using the scheme of the present embodiment, theoretically electrochemistry captures CO per ton2Energy consumption be only 322.885kWh.In electrolytic process,
The CO that the argon gas of 20mL/min will desorb in anolyte is passed through into anode liquid storage tank2It carries into gas-chromatography, verifying solution
That be sucked out is CO2Anode output CO is detected while gas2Purity.Simultaneously by low concentration CO2(CO2=10%, N2=90%)
It is passed through in catholyte with the speed of 5mL/min and carries out CO2Absorbing reaction, and CO will be absorbed2Tail gas afterwards is passed through gas-chromatography
In, verifying cathode generates and can be used to absorb CO2Ammonia spirit.
Gas-chromatography ingredient is detected to the GC of electrolyzer outlet gas the result shows that, after impressed current starts reaction, sun
Polar region can detecte apparent CO2Peak and and other gases are not detected, it was confirmed that desorbed the CO of 100% purity2；Yin
CO in the exit gas of pole2Relative amount be greatly reduced, be detected simultaneously by H2Generation, illustrate low concentration CO2It is absorbed.
Example 3
By anolyte (2M (NH4)2SO4+2MNH4HCO3) and catholyte (2M (NH4)2SO4) it is placed in the closed storage tank of 200mL
In, by pumping between electrolytic cell assembly and storage tank with the flow velocity circulation of 10mL/min, and 15mL/ is passed through to hydrogen area
The H of min2.Apply DC power supply between anode electrode and cathode electrode, cell reaction using external dc power supply (IT6932A,
Itech it) powers, electrolyzer temperature is 45 DEG C.
Current density is set as 10mA/m2, decomposition voltage at this time is 0.45V.Therefore, according to formula (7) calculation shows that:
Using the scheme of the present embodiment, theoretically electrochemistry captures CO per ton2Energy consumption be only 274.148kWh.In electrolytic process,
The CO that the argon gas of 20mL/min will desorb in anolyte is passed through into anode liquid storage tank2It carries into gas-chromatography, verifying solution
That be sucked out is CO2Anode output CO is detected while gas2Purity.Simultaneously by low concentration CO2(CO2=15%, N2=85%)
It is passed through in catholyte with the speed of 5mL/min and carries out CO2Absorbing reaction, and CO will be absorbed2Tail gas afterwards is passed through gas-chromatography
In, verifying cathode generates and can be used to absorb CO2Ammonia spirit.
Gas-chromatography ingredient is detected to the GC of electrolyzer outlet gas the result shows that, after impressed current starts reaction, sun
Polar region can detecte apparent CO2Peak and and other gases are not detected, it was confirmed that desorbed the CO of 100% purity2；Yin
CO in the exit gas of pole2Relative amount be greatly reduced, be detected simultaneously by H2Generation, illustrate low concentration CO2It is absorbed.
The influence of the U-I curve of different supporting electrolytes
In membrane electrolysis cells, by ionic conduction current.Therefore efficient fortune of the good solution conductivity to membrane electrolysis cells
Row is most important, needs that supporting electrolyte is added to improve the electric conductivity of solution in yin-yang area.In same NH4 +Under intensity, I
With 2MNH4Cl, 1M (NH4)2SO4With 2M CH3COONH4Respectively as supporting electrolyte.Ensuring various supporting electrolyte tools
There is same NH4 +When intensity, influence of the various supporting electrolytes to electrolysis performance is studied.When Fig. 5 illustrates 15 DEG C, using different branch
Hold U-I curve when electrolyte.As seen from the figure, it just can react when voltage is only 0.3V, while use is not of the same race
Class supporting electrolyte can have an impact the effect of electrolysis, generally speaking: NH4Cl > (NH4)2SO4> CH3COONH4.It considers
Cl- can accelerate the intercrystalline corrosion and spot corrosion of stainless steel, bring potential hazard for practical application.Therefore, (NH is selected4)2SO4As
Supporting electrolyte.
The U-I curve of various concentration supporting electrolyte
At determination (NH4)2SO4After supporting electrolyte, various concentration (NH is had studied4)2SO4To the shadow of electrolysis effectiveness
It rings.When Fig. 6 illustrates 15 DEG C, (the NH of various concentration4)2SO4As the U-I curve after supporting electrolyte.It can from figure
Out, (the NH of addition4)2SO4Concentration is higher, and current density is higher.In the voltage for being similarly 0.9V, when current density is from 0M
0.043A/cm20.062A/cm when 1M is risen to2, ascensional range reached 44.2%.In view of excessively high (NH4)2SO4
Concentration may influence ammonium hydroxide and absorb CO2Generate NH4HCO3Reaction balance, cause unit volume absorb CO2Amount reduce.Therefore,
We use (the NH of 1M4)2SO4 is as supporting electrolyte, and the NH being added4HCO3Concentration be also 1M, so, anode region branch
Hold electrolyte (NH4)2SO4, cathodic region supporting electrolyte (NH4)2SO4And anode region electrolyte NH4HCO3Optimal molar concentration
Than for 1:1:1
Temperature is electrolysed trapping CO to film2Influence
The rate of electrochemical reaction can be accelerated by increasing temperature.In order to verify the CO that temperature promotes film electrolysis2It trapped
The influence of journey tests the U-I curve under different temperatures, as shown in Figure 7.It can be seen from figure 7 that as the temperature rises,
Electrolysis rate is accelerated therewith.In order to reach 0.05A/cm2Current density, 15 DEG C of whens need to provide the voltage of 0.82V, and 50
DEG C when only need 0.71V.The energy consumption of electrolytic process is directly proportional to decomposition voltage, that is to say, that is maintaining 0.05A/cm2Electric current
When density, when 50 DEG C of electrolysis energy consumption is only 15 DEG C 86.6%.In view of coal-fired plant flue gas temperature with higher (is more than
100 DEG C), and this part waste heat is current and could not be effectively utilized.Thus, the waste heat of flue gas be just used on and electrolyte into
Row heat exchange is not required to external energy for heating electrolyte.However, the NH that excessively high temperature can be such that cathodic region generates3·H2O with
H2Evolution, to reduce the current efficiency in film electrolysis cathode area.After comprehensively considering, the operation temperature of electrolytic cell is maintained 45~
55 DEG C will preferably select.
The foregoing is merely presently preferred embodiments of the present invention, is not intended to limit the invention, it is all in spirit of the invention and
Made any modifications, equivalent replacements, and improvements etc., should all be included in the protection scope of the present invention within principle.
Claims (9)
1. a kind of film electrolysis promotes low concentration CO2The method of electrochemistry trapping, which is characterized in that including absorption and desorption:
It is described to be absorbed as under film electrolysis, ammonium hydroxide is absorbed into low concentration CO2The NH generated afterwards4HCO3As electrolyte, electrolysis
The NH of generation4 +OH with water power from generation-In conjunction with generation NH3·H2O, circulation is as capture low concentration CO2Absorbing liquid；
The desorption is the NH under film electrolysis4HCO3It is electrolysed the HCO generated3 -H with water power from generation+It is high-purity in conjunction with generating
Spend CO2；
The low concentration CO2Concentration be 10~20%, the high-purity CO2Concentration be 100%.
2. a kind of film electrolysis promotes low concentration CO as described in claim 12The method of electrochemistry trapping, which is characterized in that the side
Method is that cation-exchange membrane is placed in electrolytic cell to be classified as anode region and cathodic region, and NH is added in anode region4HCO3Solution, yin
Polar region is passed through low concentration CO2, and apply DC power supply between anode electrode and cathode electrode:
Under the action of electric current, H of the water power from generation+With the NH in anolyte4HCO3Reaction releases the CO of high-purity2, simultaneously
Generate NH4 +；NH4 +The OH of cathodic region and water power from generation is reached through cation-exchange membrane-In conjunction with generation NH3·H2O, for catching
It catches and absorbs low concentration CO2, and by the NH of generation4HCO3It is recycled back to anode region.
3. a kind of film electrolysis promotes low concentration CO as claimed in claim 22The method of electrochemistry trapping, which is characterized in that the electricity
The temperature for solving slot is 45~55 DEG C.
4. a kind of film electrolysis promotes low concentration CO as claimed in claim 22The method of electrochemistry trapping, which is characterized in that the sun
Pole electrode is hydrogen diffusion electrode, and the cathode electrode is foam nickel electrode.
5. a kind of film electrolysis promotes low concentration CO as claimed in claim 22The method of electrochemistry trapping, which is characterized in that the sun
Polar region is passed through hydrogen, and hydrogen is oxidized to H on the anode electrode+。
6. a kind of film electrolysis promotes low concentration CO as claimed in claim 52The method of electrochemistry trapping, which is characterized in that the hydrogen
Gas is precipitated by cathodic region, and is recycled back to cathodic region by hydrogen storage tank.
7. a kind of film electrolysis promotes low concentration CO as claimed in claim 22The method of electrochemistry trapping, which is characterized in that the sun
Polar region and cathodic region also need that supporting electrolyte (NH is added4)2SO4。
8. a kind of film electrolysis promotes low concentration CO as claimed in claim 72The method of electrochemistry trapping, which is characterized in that the sun
Polar region (NH4)2SO4, cathodic region (NH4)2SO4And anode region electrolyte NH4HCO3Molar concentration rate be 1:1:1.
9. a kind of film electrolysis promotes low concentration CO as claimed in claim 22The method of electrochemistry trapping, which is characterized in that anode
Area, cathodic region solution using corresponding solution reservoir store, and by circulating pump make solution anode region, cathodic region with it is corresponding
Storage tank between recycle.
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